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Title: High-Density Ultra-small Clusters and Single-Atom Fe Sites Embedded in Graphitic Carbon Nitride (g-C3N4) for Highly Efficient Catalytic Advanced Oxidation Processes

Abstract

Ultra-small metal clusters have attracted great attention owing to their superior catalytic performance and extensive application in heterogeneous catalysis. However, the synthesis of high-density metal clusters is very challenging due to their facile aggregation. In this work, one-step pyrolysis was used to synthesize ultra-small clusters and single-atom Fe sites embedded in graphitic carbon nitride with high density (iron loading up to 18.2 wt %), evidenced by high-angle annular dark field-scanning transmission electron microscopy, X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, and 57Fe Mössbauer spectroscopy. The catalysts exhibit enhanced activity and stability in degrading various organic samples in advanced oxidation processes. The drastically increased metal site density and stability provide useful insights into the design and synthesis of cluster catalysts for practical application in catalytic oxidation reactions.

Authors:
 [1]; ORCiD logo [2];  [1];  [3];  [1]; ORCiD logo [4];  [5];  [6]; ORCiD logo [6]; ORCiD logo [1]
  1. Dalian Univ. of Technology (People's Republic of China)
  2. Davidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, United States
  3. Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, PR China
  4. Dalian Univ. of Technology (People's Republic of China); Pennsylvania State Univ., University Park, PA (United States)
  5. Purdue Univ., West Lafayette, IN (United States)
  6. Chinese Academy of Sciences (CAS), Dalian (PR China). Dalian Inst. of Chemical Physics
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
National Natural Science Foundation of China (NSFC); Fundamental Research Funds for the Central Universities; Qianren Program of China; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES); Canadian Light Source
OSTI Identifier:
1476106
Grant/Contract Number:  
21401017; 21236008; DUT16LK12; AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 12; Journal Issue: 9; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
ENGLISH
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; ultra-small clusters; single atoms; FeNx/g-C3N4; high-density; AOPs

Citation Formats

An, Sufeng, Zhang, Guanghui, Wang, Tingwen, Zhang, Wenna, Li, Keyan, Song, Chunshan, Miller, Jeffrey T., Miao, Shu, Wang, Junhu, and Guo, Xinwen. High-Density Ultra-small Clusters and Single-Atom Fe Sites Embedded in Graphitic Carbon Nitride (g-C3N4) for Highly Efficient Catalytic Advanced Oxidation Processes. United States: N. p., 2018. Web. doi:10.1021/acsnano.8b04693.
An, Sufeng, Zhang, Guanghui, Wang, Tingwen, Zhang, Wenna, Li, Keyan, Song, Chunshan, Miller, Jeffrey T., Miao, Shu, Wang, Junhu, & Guo, Xinwen. High-Density Ultra-small Clusters and Single-Atom Fe Sites Embedded in Graphitic Carbon Nitride (g-C3N4) for Highly Efficient Catalytic Advanced Oxidation Processes. United States. https://doi.org/10.1021/acsnano.8b04693
An, Sufeng, Zhang, Guanghui, Wang, Tingwen, Zhang, Wenna, Li, Keyan, Song, Chunshan, Miller, Jeffrey T., Miao, Shu, Wang, Junhu, and Guo, Xinwen. 2018. "High-Density Ultra-small Clusters and Single-Atom Fe Sites Embedded in Graphitic Carbon Nitride (g-C3N4) for Highly Efficient Catalytic Advanced Oxidation Processes". United States. https://doi.org/10.1021/acsnano.8b04693. https://www.osti.gov/servlets/purl/1476106.
@article{osti_1476106,
title = {High-Density Ultra-small Clusters and Single-Atom Fe Sites Embedded in Graphitic Carbon Nitride (g-C3N4) for Highly Efficient Catalytic Advanced Oxidation Processes},
author = {An, Sufeng and Zhang, Guanghui and Wang, Tingwen and Zhang, Wenna and Li, Keyan and Song, Chunshan and Miller, Jeffrey T. and Miao, Shu and Wang, Junhu and Guo, Xinwen},
abstractNote = {Ultra-small metal clusters have attracted great attention owing to their superior catalytic performance and extensive application in heterogeneous catalysis. However, the synthesis of high-density metal clusters is very challenging due to their facile aggregation. In this work, one-step pyrolysis was used to synthesize ultra-small clusters and single-atom Fe sites embedded in graphitic carbon nitride with high density (iron loading up to 18.2 wt %), evidenced by high-angle annular dark field-scanning transmission electron microscopy, X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, and 57Fe Mössbauer spectroscopy. The catalysts exhibit enhanced activity and stability in degrading various organic samples in advanced oxidation processes. The drastically increased metal site density and stability provide useful insights into the design and synthesis of cluster catalysts for practical application in catalytic oxidation reactions.},
doi = {10.1021/acsnano.8b04693},
url = {https://www.osti.gov/biblio/1476106}, journal = {ACS Nano},
issn = {1936-0851},
number = 9,
volume = 12,
place = {United States},
year = {Wed Sep 05 00:00:00 EDT 2018},
month = {Wed Sep 05 00:00:00 EDT 2018}
}

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Free Publicly Available Full Text
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Cited by: 320 works
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Figures / Tables:

Figure 1 Figure 1: Optimized structures of various positions of single Fe atom and Fe cluster in g-C3N4. (a) Single Fe atom in the center of six-fold cavity, (b) single Fe atom in interlayer, (c) Fe cluster in interlayer (Site1), (d) Fe cluster in interlayer (Site2), (e) Fe cluster in interlayer (Site3).

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.